Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics

Autor: A. C. LaForge, R. Michiels, Y. Ovcharenko, A. Ngai, J. M. Escartín, N. Berrah, C. Callegari, A. Clark, M. Coreno, R. Cucini, M. Di Fraia, M. Drabbels, E. Fasshauer, P. Finetti, L. Giannessi, C. Grazioli, D. Iablonskyi, B. Langbehn, T. Nishiyama, V. Oliver, P. Piseri, O. Plekan, K. C. Prince, D. Rupp, S. Stranges, K. Ueda, N. Sisourat, J. Eloranta, M. Pi, M. Barranco, F. Stienkemeier, T. Möller, M. Mudrich
Jazyk: angličtina
Rok vydání: 2021
Předmět:
Zdroj: Physical Review X, Vol 11, Iss 2, p 021011 (2021)
Druh dokumentu: article
ISSN: 2160-3308
DOI: 10.1103/PhysRevX.11.021011
Popis: Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation; therefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we directly measure the timescale of interatomic Coulombic decay (ICD) in resonantly excited helium nanodroplets using a high-resolution, tunable, extreme ultraviolet free-electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprisingly fast, with decay times as short as 400 fs, nearly independent of the density of the excited states. Using a combination of time-dependent density functional theory and ab initio quantum chemistry calculations, we elucidate the mechanisms of this ultrafast decay process, where pairs of excited helium atoms in one droplet strongly attract each other and form merging void bubbles, which drastically accelerates ICD.
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